Some indanone based NLO-phores in the form of donor-spacer-acceptor dyads has been synthesized by knovenagel condensation. H-1 and C-13 NMR, FT-IR, CHN analysis along with atomic absorption and MASS spectroscopy supported the predicted structure of the products. Electrochemical, photochemical and photophysical properties of these compounds were investigated. The third order nonlinear refractive index, n(2), and nonlinear absorption coefficient, beta, of synthesized chromophores were assessed by the open and closed aperture Z-scan measurements, respectively. The quantum chemistry study was performed on synthesized compounds with the OFT approach. The theoretical and experimental results show that these compounds can be considered as candidates to be used in optical applications. (C) 2017 Elsevier B.V. All rights reserved.